In recent studies of bulk metallic glasses (BMGs), the serrated behavior attracts more attention, since they are similar to the Portevin–Le Chatelier (PLC) effect found in crystalline materials. With the absence of solute atoms and dislocations, the serration was attributed to the shear-band operations during the deformation for BMGs. However, due to the intrinsically-brittle property for most BMGs, the serrated behavior is always omitted and the emphasis is placed on the catastrophic fracture. The present study unitizes the geometrical constraints to investigate the serrated behavior under different loading modes, i.e., the compression and nanoindentation experiments. The features of shear bands after deformation were characterized, and the serrated behavior was compared between these two loading modes. Furthermore, a theoretical model was applied on the analysis of characteristics of serration behavior.